Doctor of Philosophy / Department of Physics / Chii-Dong Lin / Imaging of molecules has always occupied an essential role in physical, chemical and biological sciences. X-ray and electron diffraction methods routinely achieve sub-angstrom spatial resolutions but are limited to probing dynamical timescales longer than a picosecond. With the advent of femtosecond intense lasers, a new imaging paradigm emerges in last decade based on laser-induced electron diffraction (LIED). It has been placed on a firm foundation by the quantitative rescattering theory, which established that large-angle e-ion elastic differential cross sections (DCS) can be retrieved from the LIED spectrum. We further demonstrate that atomic potentials can be accurately retrieved from those extracted DCSs at energies from a few to several tens of electron volts. Extending to molecules, we show mid-infrared (mid-IR) lasers are crucial to generate high-energy electron wavepackets (> 100 eV) to resolve the atomic positions in a molecule. These laser-driven 100 eV electrons can incur core-penetrating collisions where the momentum transfer is comparable to those attained in conventional keV electron diffraction. Thus a simple independent atom model (IAM), which has been widely used in conventional electron diffractions, may apply for LIED. We theoretically examine and validate the applicability of IAM for electron energies above 100 eV using e-molecule large-angle collision data obtained in conventional experiments, demonstrating its resolving powers for bond lengths about 0.05 angstrom. The Validity of IAM is also checked by an experimental LIED investigation of rare gas atoms in the mid-IR regime. We show that the electron’s high energy promotes core-penetrating collisions at large scattering angles, where the e-atom interaction is dominated by the strong short range atomic-like potential. Finally, we analyze the measured LIED spectrum of N[subscript]2 and O[subscript]2 at three mid-IR wavelengths (1.7, 2.0, and 2.3 μm). As expected, the retrieved bond lengths of N[subscript]2 at three wavelengths are about same as the equilibrium N[subscript]2 bond length. For O[subscript]2, the data is also consistent with a bond length contraction of 0.1 angstrom within 4-6 fs after tunnel ionization. This investigation establishes a foundation for this novel imaging method for spatiotemporal imaging of gas-phase molecules at the atomic scale.

This thesis presents a series of electron impact ionization measurements on the gas phase targets of argon and krypton. The (e,2e) coincidence technique has been employed to measure the triple differential cross section (TDCS) using a new coincidence spectrometer designed to operate in the low energy regime (2 to 5 times the ionization energy) and in the coplanar geometry. The spectrometer is a conventional device utilizing a non-energy selected electron gun and two 1800 hemispherical electron analysers fitted with channel electron multipliers for detection of the outgoing electrons. A series of TDCS measurements were performed on the 3s inner-valence and 3p valence orbitals of argon employing coplanar asymmetric kinematics. Measurements for both orbitals were performed at an incident energy of 113.5 eV, ejected energies of 10, 7.5, 5 and 2 eV and a scattering angle of -15°. The energy of the scattered electron in each case was chosen to satis~' energy conservation and is dependent on the ionization energies of the different orbitals. The experimental cross sections are compared to theoretical TDCS calculations using the distorted wave Born approximation (DWBA) and variations of the DWBA in an attempt to investigate the role that post collisional interaction (PCI), polarization and electron exchange play in describing the TDCS in the low energy regime. To further extend this analysis, a series of TDCS measurements were performed on the 3s and 4s. orbitals of argon and krypton, respectively, employing coplanar symmetric kinematics. Measurements were performed for the 3s orbital at outgoing energies of 50, 20, 10 and 4eV and for the 4s orbital at outgoing energies of 85, 50, 20 and 10 eV. The kinematics were chosen to coincide with several of the (e,2e) measurements made in the same geometry on the 3p orbital of argon by Rouvellou et al (1998). The experimental results were again compared to a DWBA calculation and similar variations to those employed for the asymmetric measurements.

Nous avons étudié la structure de la surface de mica muscovite clivée à l?air par diffraction d?électrons lents en mode oscillant. Cette nouvelle méthode d?analyse structurale, que nous avons développée à partir d?un système optique standard de résolution conventionnelle, possède une grande sensibilité. En outre, elle permet de former des images de diffraction entières sans procéder, comme le font les autres diffractomètres à haute résolution, à une reconstitution ligne par ligne. Cette caractéristique permet aussi de réaliser des acquisitions d?image qui sont corrélées temporellement avec une excitation extérieure, ce qui rend possible toute une gamme d?expériences nouvelles, notamment dans le cadre de la réponse thermodynamique d?une surface au voisinage d?une transition de phase. Notre étude de la surface du mica muscovite par diffraction d?électrons lents en mode oscillant a permis pour la première fois de mettre en évidence la nanostructuration de sa couche superficielle. Notre interprétation est que lors du clivage, la surface du mica s?auto-organise pour former un arrangement d?îlots à l?intérieur desquels les atomes de potassium occupent les sites réguliers du cristal. Les îlots sont soit de taille définie soit séparés par une distance définie. Dans les zones interstitielles qui les séparent, les ions potassium, en concentration beaucoup plus faible, formeraient une couche amorphe.

No description available.

Thesis (Ph. D.)--University of Missouri-Columbia, 1997. / Typescript. Vita. Includes bibliographical references (leaves 197-202). Also available on the Internet.

Thesis (Ph. D.)--University of Missouri-Columbia, 1997. / Typescript. Vita. Includes bibliographical references (leaves 197-202). Also available on the Internet.

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Made available in DSpace on 2014-10-09T12:43:57Z (GMT). No. of bitstreams: 0 / Made available in DSpace on 2014-10-09T14:08:19Z (GMT). No. of bitstreams: 1 06781.pdf: 5180316 bytes, checksum: 400f92bad2534a326e86a6f14c3ba5cb (MD5) / Dissertacao (Mestrado) / IPEN/D / Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP

Submitted by Claudinei Pracidelli (cpracide@ipen.br) on 2016-06-22T12:43:46Z No. of bitstreams: 0 / Made available in DSpace on 2016-06-22T12:43:46Z (GMT). No. of bitstreams: 0 / Neste trabalho foi estabelecido um sistema padrão primário para raios X de energias baixas (10 kV a 50 kV), utilizando uma câmara de ionização de ar livre de cilindros concêntricos da marca Victoreen (modelo 481-5) no Laboratório de Calibração de Instrumentos (LCI) do Instituto de Pesquisas Energéticas e Nucleares (IPEN/CNEN-SP). Para isso foi desenvolvido um novo protocolo de alinhamento da câmara de ionização no sistema de radiação e foi feita uma modificação no suporte dos micrômetros utilizados para o movimento dos cilindros internos. Os resultados obtidos nos testes de estabilidade e de caracterização ficaram dentro dos limites estabelecidos pelas normas IEC 61674 e IEC 60731. Foram determinados também os fatores de correção para atenuação de fótons no ar, transmissão e espalhamento no diafragma, espalhamento e fluorescência, e recombinação iônica. Esses valores foram comparados com os valores obtidos pelo laboratório padrão primário alemão,Physikalisch-Technische Bundesanstalt (PTB), mostrando boa concordância. Por último, foi determinado o valor absoluto da grandeza taxa de kerma no ar para as qualidades padronizadas de mamografia de feixes diretos WMV28 e WMV35 e feixes atenuados WMH28 e WMH35; os resultados são compatíveis, com diferença máxima de 3,8% com os valores obtidos utilizando o sistema padrão secundário do LCI. / Dissertação (Mestrado em Tecnologia Nuclear) / IPEN/D / Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP